Measurements of the C-13 NMR spectrum, spin-lattice, and spin-spin rel
axation rates in K3C60 reveal the existence of two distinct molecular
motions of the same C60 molecule above 200 K, with respective activati
on energies of 2600 +/- 300 and 6800 +/- 500 K. We propose a simple mo
del to explain these data implying fast axial jump rotation of the C60
molecules combined with slow jumps around perpendicular axes. The ana
lysis of the spectra indicates an abrupt change in the molecular motio
n below 200 K suggestive of a phase transition also evidenced by calor
imetric measurements.